Direct Formation of the Atomic Pd-ZnO Interface by Magnetron Sputtering Primed for Methanol Production from CO2

Abstract

Carbon dioxide is not only a greenhouse gas but also a valuable feedstock for producing chemicals and fuels, especially methanol, which serves as an energy storage medium and a precursor for olefins and gasoline. Herein, we show that a clean, atomically defined interface between a Pd catalyst and a ZnO support allows for the direct production of methanol from CO2without any catalyst activation or induction period. Using magnetron sputtering, Pd atoms are directly deposited onto the ZnO surface, self-assembling into Pd nanoclusters with a high fraction of surface atoms, driven solely by the surface chemistry of ZnO, eliminating the need for solvents, reagents, or ligands. This atomically defined Pd/ZnO interface facilitates Pd–Zn alloying in situ during the reaction, achieving an impressive methanol production rate of 16.4 mol h–1mol–1Pd, outperforming catalysts prepared by other methods. By eliminating interfacial impurities and the consequent need for pretreatment, our work establishes magnetron sputtering as a transformative method for fabricating high-performance catalysts.